Process for lanthanide and actinide metals ore reduction

ABSTRACT

The Lanthanide and Actinide series of metals are found mainly in the three ores Monazite, Carnotite, and Uraninite or Pitchblende. In winning these metals from the ores usually the oxides are separated either seperately or in groups first, then the oxides are reduced either separately or in groups, thereby providing individual metals, or an alloy known as a commercially designated Misch metal. Such separations and reductions apply to only the ores as found natural and does not include the manmade nuclear transformation elements of the series. The separations and reductions both from the ores, the oxides, and the Misch metal are quite complicated, cumbersome, costly, and at times are inefficient. By application of the instant process such ores and oxides may be reduced in either of those forms in a more simple manner to either the individual metals or the alloy. The alloy metal may then be subsequently separated into individual metals at great savings in operations and cost in comparison to that which is known. The ores or oxides are subjected to a certain liquid formula solution, such material being finely pulverized, by mixing together within a suitable container, followed by additions of pulverized limestone and stirred while the reaction goes to completion. The liquid formula is comprised of phosphoric acid, zinc oxide, and an alkylphenol polyglycol ether type sulfated surfactant. The mixture is heated within the container by an endothermic heat source until the ore has been digested by the liquid formula solution with the consequent release of gases and expanded in volume to a dry, spongelike state. In this condition the material is considered as being &#39;&#39;&#39;&#39;fixed&#39;&#39;&#39;&#39; for smelting. Upon smelting the material releases the metal which forms into ingot-like masses at the bottom of the furnace as reduced and smelted metal. The combination of reduction ingredients are effective, therefore, in liberating the metals from chemically bound oxygen and other impurities upon heating the mixture and then smelting the residue.

United gtates Fatent [191 Taylor [451 Feb. 12, 1974 PROCESS FORLANTHANIDE AND ACTINIDE METALS ()RE REDUCTION Paul Franklin Taylor, PO.Box 468, Crossville, Tenn. 38555 [22] Filed: Dec. 13, 1972 [21] Appl.No.: 314,809

[76] Inventor:

[52] US. Cl 75/841 R, 75/84, 75/101 R, 75/108, 252/301.1 R, 423/18,423/19,

[51] Int. Cl. C22c 59/00, C220 61/04 [58] Field of Search 423/18, 19,20, 21; 252/301.l R; 75/84, 84.1 R, 101, 108

[56] References Cited UNITED STATES PATENTS 12/1958 Long 423/18 11/1958Bailes et a1. 423/18 Primary Examiner-Benjamin R. Padgett AssistantExaminerB. Hunt [57] ABSTRACT reductions apply to only the ores as foundnatural and does not include the manmade nuclear transformation elementsof the series. The separations and reductions both from the ores, theoxides, and the Misch metal are quite complicated, cumbersome, costly,and at times are inefficient. By application of the instant process suchores and oxides may be reduced in either of those forms in a more simplemanner to either the individual metals or the alloy. The alloy metal maythen be subsequently separated into individual metals at great savingsin operations and cost in comparison to that which is known. The ores oroxides are subjected to a certain liquid formula solution, such materialbeing finely pulverized, by mixing together within a suitable container,followed by additions of pulverized limestone and stirred while thereaction goes to completion. The liquid formula is comprised ofphosphoric acid, zinc oxide, and an alkylphenol polyglycol ether typesulfated surfactant. The mixture is heated within the container by anendothermic heat source until the ore has been digested by the liquidformula solution with the consequent release of gases and expanded involume to a dry, spongelike state. In this condition the material isconsidered as being fixed for smelting. Upon smelting the materialreleases the metal which forms into ingot-like masses at the bottom ofthe furnace as reduced and smelted metal. The combination of reductioningredients are effective, therefore, in liberating the metals fromchemically bound oxygen and other impurities upon heating the mixtureand then smelting the residue.

3 Claims, No Drawings The ore is of the following types or the materialfromwhich the metallic oxides are derived; Monazite, Carnotite andUraninite or Pitchblende. The liquid formula chemical solution is of thefollowing composition (by weight ratio);

24.20 No. more or less 0.50 No. more or less 1.00 No. more or lessPhosphoric acid Zinc Oxide Sulfated Surfactant The sulfated surfactantis a type of wetting agent and of composition alkylphenol polyglycolether. The powdered calcium carbonate (CaCO should be at least 99percent pure.

When the selected ore material and other starting materials are mixedtogether within a common container and heated with endothermic heat,oxygen and other impurities separate from the metals and form intochemical union with the liquid chemical solution formula and calciumoxide of the limestone, part of which is expelled in the form of gases.The metals are then smelted out to ingot form from the residue material.

It is, therefore, an object of the present invention process to provideanother method for the production of Lanthanide and Actinide metals.

It is another object of the present invention process to provide amethod for producing those metals by utilizing either the ores or theoxides derived therefrom with the process, and subsequent smelting.

It is a further object of the present invention process to provide amore simple and economical manner for producing these metals.

Other objects and advantages of the present invention process willbecome apparent from a further reading of the description and theappended claims.

With the above and other objects in view, the present invention processmainly comprises a process for separating the Lanthanide and Actinideseries of metals from chemically combined oxygen and other impurities,featuring ease of reduction operations, and one that is economicallyadvantageous.

The process begins with the stated mixing together of the startingmaterials in a suitable pot or vat, followed by stirring until thevisible chemical reaction is completed and the oxide impurities broughtinto solution.

The pot or vat is then placed within a suitable furnace arrangementwhere effective heat may be applied to it.

The solution with the ore is then boiled with heat until sufficientliquid has digested the ore with the release of some gases. The boilingis attended and enhanced by frequent stirrings with a suitable agitator.It is also attended by such mechanical arrangements as necessary for thecollecting and venting of gases.

The temperature operation range throughout the boiling period is thatwhich is necessary for maintaining a gentle rolling boil. Heating isterminated when residue has baked to a dry and expanded solid state.

The resulting residue may then be smelted and/or refined by conventionalmeans to produce Lanthanide and Actinide series metal. For thatoperation residue is pulverized to necessary chunk sizes to suit thefurnace smelting technique requirements.

OPERATIONAL EXAMPLE The operation for Lanthanide and Actinide metal orereduction as derived from the foregoing specification may be exemplifiedmore particularly by an explanation for the reduction of seventy gramsof commercially pure thorium dioxide (ThO which the inventor hasoperated successfully. The oxide is as fine or finer than 325 mesh.

The reduction equipment consists of the following: A silicon heatresisting non-corroding pint crucible, a non-corroding stirring rod, andan appropiate gas-type or electric heat source.

Introduced within the crucible are the seventy grams of the thoriumdioxide, or one volume measure, two volume measures of the abovedescribed liquid chemical solution formula known as Taylor formula, suchsolution being comprised of ingredients as described, and one-eighthvolume measure of limestone of approximately mesh in particle size, thelimestone being at least 99 percent pure calcium carbonate (CaCO Thedioxide, solution formula and limestone are thoroughly stirred and mixeduntil the visible reaction of the release of gases has terminated.

With the crucible resting on the gas-type or electric heat source gentleheat is applied until boiling commences. The heat is then regulated sothat a very gentle rolling boil continues. A proper vent is required forthe outgassing fumes. The boiling is continued until the residue isbaked to a dry solid state. During boiling the mixture is stirred asoften as necessary to maintain a homogeneous state.

Upon termination of boiling the residue is allowed to cool and thenremoved and pulverized as necessary for entry into the smelting and/orrefining furnace.

A second operational example utilizing Monazite ore of a pureconcentrated form and pulverized to -325 mesh is conducted exactly asthe above example except the one volume measure of the ore weighs 82grams instead of the seventy of the thorium dioxide, and serves as anexample in reason for mixing the various ores and oxides with solutionand limestone by volume measurement instead of by weight measurement,with heavier pulverized ore not requiring more or less solution andlimestone than the thorium dioxide example for the necessary reduction,and such also is true with lighter ores. Thus, the necessary ore,solution and limestone ratios are more important relative to volumemeasurement than by weight, and so the above example ratios present anorm in the reduction of the Lanthanide and Actinide concentrated oresor the oxides derived from them, but is not intended to mean thereduction effectiveness for these metal series is confined to an exactand definite ratio either by weight or by volume, as different meshsizes of both the ore, their oxides and the limestone changes theweights while the volumes remain constant.

What is claimed as new and desired to be secured by Letters Patent is:

. 3 1. A method of reducing Lanthanide and Actinide series metal ore orthe oxide derived from them to ingot or alloy forms comprising the stepsof:

C. Bringing the mixture to a boil while stirring to obtain a homogeneoussolution,

D. vaporizing the volatile materials until residue is baked to a drysolid state,

E. Smelting the remaining residue to produce Lanthanide and Actinideseries metal ingots or alloy.

2. The process of claim number one wherein the Lanthanide and Actinideseries metal ore is in the form of Monazite, Carnotite, and Uraninite orPitchblende, or

the oxides derived from them.

3. The process of claim number one wherein the sulfated surfactant is analkylphenol polyglycol ether.

2. The process of claim number one wherein the Lanthanide and Actinideseries metal ore is in the form of Monazite, Carnotite, and Uraninite orPitchblende, or the oxides derived from them.
 3. The process of claimnumber one wherein the sulfated surfactant is an alkylphenol polyglycolether.